Ca_1-xLixAl_1-xSi_1+xN₃:Eu²⁺ solid solutions as broadband, color-tunable and thermally robust red phosphors for superior color rendition white light-emitting diodes

Color rendition, luminous efficacy and reliability are three key technical parameters for white light-emitting diodes (wLEDs) that are dominantly determined by down-conversion phosphors. However, there is usually an inevitable trade-off between color rendition and luminescence efficacy because the spectrum of red phosphor (that is, spectral broadness and position) cannot satisfy them simultaneously. In this work, we report a very promising red phosphor that can minimize the aforementioned trade-off via structure and band-gap engineering, achieved by introducing isostructural LiSi2N3 into CaAlSiN₃:Eu²⁺. The solid solution phosphors show both substantial spectra broadening (88→117 nm) and blueshift (652→642 nm), along with a significant improvement in thermal quenching (only a 6% reduction at 150 °C), which are strongly associated with electronic and crystal structure evolutions. The broadband and robust red phosphor thus enables fabrication of super-high color rendering wLEDs (Ra=95 and R9=96) concurrently with the maintenance of a high-luminous efficacy (101 lm W- 1), validating its superiority in highperformance solid state lightings over currently used red phosphors.